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Depends on where the bottleneck lies. If it is reading from disk, then no. If it is on the computation of the md5 hashes, then possibly yes, by implementing the hash algorithm on the GPU.

I would suggest trying to optimize on the CPU first (i.e. batch multiple entries and distribute to multiple CPU threads). If that still doesn't give you the performance you need, then you can use OpenTK+GLSL or Cloo+OpenCL to speed up the algorithm.

Thank you for the response! Yeah I'm specifically looking to offload the hashing to the GPU. Is there already a HashMD5(text) function somewhere in one of the libraries that you know of? I'm sure someone, somewhere has had a similar situation.

http://majuric.org/software/cudamd5/ Supposedly works on CUDA(nVidia cards), so you can either try to port the code to OpenCL or use a CUDA.Net binding.
There are probably more sources out there, I didnt google for very long.

It would be nice to add OpenCL capabilities to OpenTK. In fact, there is already code for this in the binding generator.

The idea is to convert the .h files to xml via Generator.Convert and then pass that to Generator.Bind to generate the actual bindings. This entails some amount of manual work to define enumerations, but it is certainly doable (and the specs are much smaller than even OpenGL ES 1.1)